Microscopic electronic configurations after ultrafast magnetization dynamics

We provide a model for the prediction of the electronic and magnetic configurations of ferromagnetic Fe after an ultrafast decrease or increase of magnetization. The model is based on the well-grounded assumption that, after the ultrafast magnetization change, the system achieves a partial thermal equilibrium. With statistical arguments it is possible to show that the magnetic configurations are qualitatively different in the case of reduced or increased magnetization. The predicted magnetic configurations are then used to compute the dielectric response at the 3p (M) absorption edge, which can be related to the changes observed in the experimental T-MOKE data. The good qualitative agreement between theory and experiment offers a substantial support to the existence of an ultrafast increase of magnetisation, which has been fiercely debated in the last years.Comment: Main text 10 pages including 7 figures. Supplemental material 5 pages including 1 figur

Microscopic origin of Heisenberg and non-Heisenberg exchange interactions in ferromagnetic bcc Fe

By means of first principles calculations we investigate the nature of exchange coupling in ferromagnetic bcc Fe on a microscopic level. Analyzing the basic electronic structure reveals a drastic difference between the $3d$ orbitals of $E_g$ and $T_{2g}$ symmetries. The latter ones define the shape of the Fermi surface, while the former ones form weakly-interacting impurity levels. We demonstrate that, as a result of this, in Fe the $T_{2g}$ orbitals participate in exchange interactions, which are only weakly dependent on the configuration of the spin moments and thus can be classified as Heisenberg-like. These couplings are shown to be driven by Fermi surface nesting. In contrast, for the $E_g$ states the Heisenberg picture breaks down, since the corresponding contribution to the exchange interactions is shown to strongly depend on the reference state they are extracted from. Our analysis of the nearest-neighbour coupling indicates that the interactions among $E_g$ states are mainly proportional to the corresponding hopping integral and thus can be attributed to be of double-exchange origin.Comment: 5 pages, 4 figure

Analytic continuation by averaging Pad\'e approximants

The ill-posed analytic continuation problem for Green's functions and self-energies is investigated by revisiting the Pad\'{e} approximants technique. We propose to remedy the well-known problems of the Pad\'{e} approximants by performing an average of several continuations, obtained by varying the number of fitted input points and Pad\'{e} coefficients independently. The suggested approach is then applied to several test cases, including Sm and Pr atomic self-energies, the Green's functions of the Hubbard model for a Bethe lattice and of the Haldane model for a nano-ribbon, as well as two special test functions. The sensitivity to numerical noise and the dependence on the precision of the numerical libraries are analysed in detail. The present approach is compared to a number of other techniques, i.e. the non-negative least-square method, the non-negative Tikhonov method and the maximum entropy method, and is shown to perform well for the chosen test cases. This conclusion holds even when the noise on the input data is increased to reach values typical for quantum Monte Carlo simulations. The ability of the algorithm to resolve fine structures is finally illustrated for two relevant test functions.Comment: 10 figure

Lattice dynamics of palladium in the presence of electronic correlations

We compute the phonon dispersion, density of states, and the Gr\"uneisen parameters of bulk palladium in the combined density functional theory (DFT) and dynamical mean-field theory (DMFT). We find good agreement with experimental results for ground state properties (equilibrium lattice parameter and bulk modulus) and the experimentally measured phonon spectra. We demonstrate that at temperatures $T \lesssim 20~K$ the phonon frequency in the vicinity of the Kohn anomaly, $\omega_{T1}({\bf q}_{K})$, strongly decreases. This is in contrast to DFT where this frequency remains essentially constant in the whole temperature range. Apparently correlation effects reduce the restoring force of the ionic displacements at low temperatures, leading to a mode softening.Comment: minor revision

Electronic and Magnetic Properties of single Fe atoms on a CuN Surface; Effects of Electron Correlations

The electronic structure and magnetic properties of a single Fe adatom on a CuN surface have been studied using density functional theory in the local spin density approximation (LSDA), the LSDA+U approach and the local density approximation plus dynamical mean-field theory (LDA+DMFT). The impurity problem in LDA+DMFT is solved through exact diagonalization and in the Hubbard-I approximation. The comparison of the one-particle spectral functions obtained from LSDA, LSDA+U and LDA+DMFT show the importance of dynamical correlations for the electronic structure of this system. Most importantly, we focused on the magnetic anisotropy and found that neither LSDA, nor LSDA+U can explain the measured, high values of the axial and transverse anisotropy parameters. Instead, the spin excitation energies obtained from our LDA+DMFT approach with exact diagonalization agree significantly better with experimental data. This affirms the importance of treating fluctuating magnetic moments through a realistic many-body treatment when describing this class of nano-magnetic systems. Moreover, it facilitates insight to the role of the hybridization with surrounding orbitals.Comment: 17 pages, 4 figure

The electronic structure of palladium in the presence of many-body effects

Including on-site electronic interactions described by the multi-orbital Hubbard model we study the correlation effects in the electronic structure of bulk palladium. We use a combined density functional and dynamical mean field theory, LDA+DMFT, based on the fluctuation exchange approximation. The agreement between the experimentally determined and the theoretical lattice constant and bulk modulus is improved when correlation effects are included. It is found that correlations modify the Fermi surface around the neck at the $L$-point while the Fermi surface tube structures show little correlation effects. At the same time we discuss the possibility of satellite formation in the high energy binding region. Spectral functions obtained within the LDA+DMFT and $GW$ methods are compared to discuss non-local correlation effects. For relatively weak interaction strength of the local Coulomb and exchange parameters spectra from LDA+DMFT shows no major difference in comparison to $GW$

Electron correlations in Mnx_xGa1−x_{1-x}As as seen by resonant electron spectroscopy and dynamical mean field theory

After two decades from the discovery of ferromagnetism in Mn-doped GaAs, its origin is still debated, and many doubts are related to the electronic structure. Here we report an experimental and theoretical study of the valence electron spectrum of Mn-doped GaAs. The experimental data are obtained through the differences between off- and on-resonance photo-emission data. The theoretical spectrum is calculated by means of a combination of density-functional theory in the local density approximation and dynamical mean-field theory (LDA+DMFT), using exact diagonalisation as impurity solver. Theory is found to accurately reproduce measured data, and illustrates the importance of correlation effects. Our results demonstrate that the Mn states extend over a broad range of energy, including the top of the valence band, and that no impurity band splits off from the valence band edge, while the induced holes seem located primarily around the Mn impurity.Comment: 5 pages, 4 figure

Operation of EMEP ‘supersites’ in the United Kingdom. Annual report for 2008.

As part of its commitment to the UN-ECE Convention on Long-range Transboundary Air Pollution the United Kingdom operates two ‘supersites’ reporting data to the Co-operative Programme for Monitoring and Evaluation of the Long-range Transmission of Air Pollutants in Europe (EMEP). This report provides the annual summary for 2008, the second full calendar year of operation of the first EMEP ‘supersite’ to be established in the United Kingdom. Detailed operational reports have been submitted to Defra every 3 months, with unratified data. This annual report contains a summary of the ratified data for 2008. The EMEP ‘supersite’ is located in central southern Scotland at Auchencorth (3.2oW, 55.8oN), a remote rural moorland site ~20 km south-west of Edinburgh. Monitoring operations started formally on 1 June 2006. In addition to measurements made specifically under this contract, the Centre for Ecology & Hydrology also acts as local site operator for measurements made under other UK monitoring networks: the Automated Urban and Rural Network (AURN), the UK Eutrophication and Acidification Network (UKEAP), the UK Hydrocarbons Network, and the UK Heavy Metals Rural Network. Some measurements were also made under the auspices of the ‘Air Pollution Deposition Processes’ contract. All these associated networks are funded by Defra. This report summarises the measurements made between January and December 2008, and presents summary statistics on average concentrations. The site is dominated by winds from the south-west, but wind direction data highlight potential sources of airborne pollutants (power stations, conurbations). The average diurnal patterns of gases and particles are consistent with those expected for a remote rural site. The frequency distributions are presented for data where there was good data capture throughout the whole period. Some components (e.g. black carbon) show log-normal frequency distributions, while other components (e.g. ozone) have more nearly normal frequency distributions. A case study is presented for a period in June 2008, showing the influence of regional air pollutants at this remote rural site. All the data reported under the contract are shown graphically in the Appendix